An efficient two-step strategy is proposed to fabricate binderless and high-performance pseudocapacitive material/carbonaceous material composite electrodes for practical applications in energy-storage power sources. Taking value of this superior architecture, we demonstrate a three-dimensional (3D) reduced graphene oxide-supported manganese hexacyanoferrate (MnHCF/rGO) hybrid electrode. Firstly, a 3D conductive rGO scaffold is constructed via electrophoretic deposition (EPD) of graphene oxide nanoplatelets (GONPs) on graphite substrate and a subsequent electrochemical reduction to enhance their electrical conductivity. Then, MnHCF nanocubes are orderly grown onto the rGO nanosheets by an anodic galvanostatic pulse electrodeposition (GPED). This 3D porous electrode structure provides more active sites for electrochemical reactions, facilitates electron and ion transport and prevents the aggregation of MnHCF nanocubes during charge-discharge cycling. The as-prepared rGO-supported MnHCF electrode demonstrates a high specific capacitance of 612 F g−1 at 1.0 A g−1 as well as outstanding cycling stability (93.8% capacitance retention after 2000 cycles). Furthermore, an asymmetric supercapacitor device consisting of the MnHCF/rGO positive electrode and pure rGO negative electrode delivers a high energy density of 45.3 Wh Kg−1 at a power density of 916 W kg−1 in the wide operation voltage of 1.9 V and remarkable cycling stability (91.2%, 4000 cycles).
